Catalytic Functionalization of Methane and Light Alkanes in Supercritical Carbon Dioxide

被引:21
作者
Angeles Fuentes, M. [1 ,2 ]
Olmos, Andrea [1 ,2 ]
Munoz, Bianca K. [3 ,4 ,5 ,6 ]
Jacob, Kane [3 ,4 ,5 ,6 ]
Gonzalez-Nunez, Elena [7 ]
Mello, Rossella [7 ]
Asensio, Gregorio [7 ]
Caballero, Ana [1 ,2 ]
Etienne, Michel [3 ,4 ,5 ,6 ]
Perez, Pedro J. [1 ,2 ]
机构
[1] Univ Huelva, Lab Catalisis Homogenea, Unidad Asociada CSIC CIQSO Ctr Invest Quim Sosten, Huelva 21007, Spain
[2] Univ Huelva, Dept Quim & Ciencia Mat, Huelva 21007, Spain
[3] CNRS, F-31077 Toulouse, France
[4] CNRS, Chim Coordinat Lab, F-31077 Toulouse, France
[5] Univ Toulouse, F-31077 Toulouse, France
[6] CNRS, Chim Coordinat Lab, UPS, INPT, F-31077 Toulouse, France
[7] Univ Valencia, Fac Farm, Dept Quim Organ, Valencia 46100, Spain
关键词
carbene insertion; C-H activation; diazo compounds; methane activation; silver catalysts; C-H BONDS; CARBENE INSERTION; ACTIVATION; OXIDATION; CONVERSION; SYSTEM; DFT;
D O I
10.1002/chem.201403217
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of catalytic methods for the effective functionalization of methane yet remains a challenge. The best system known to date is the so-called Catalytica Process based on the use of platinum catalysts to convert methane into methyl bisulfate with a TOF rate of 10(-3) s. In this contribution, we report a series of silver complexes con-taining perfluorinated tris(indazolyl) borate ligands that catalyze the functionalization of methane into ethyl propionate upon reaction with ethyl diazoacetate (EDA) by using supercritical carbon dioxide (scCO(2)) as the reaction medium. The employment of this reaction medium has also allowed the functionalization of ethane, propane, butane, and isobutane.
引用
收藏
页码:11013 / 11018
页数:6
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